MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Yongkui Liu,Fumin Wang,Xubin Zhang,Qing Zhang,Yi Zhai,Guojun Lv,Mengyao Li,Mengyue Li
Development of economic routes for synthesis of hollow titanium silicalite-1 (TS-1) zeolite is of great importance in industry. However, there are still challenges to synthesize hollow TS-1 zeolite without anatase TiO 2 . In this work, a one-step strategy without mesoporogen by the solid-phase conversion method was successfully developed to synthesize anatase-free hollow TS-1. The appropriate low amount of TPAOH (TPA/SiO 2 = 0.13) and the suitable crystallization temperature (170 °C) can not merely induce the formation of hollow structures, but also enable more titanium to enter the framework. Moreover, the transformation mechanism based on crystallization rate and dissolution rate was proposed according to the investigation of the transformation process. The hollow TS-1 with large cavities exhibits high catalytic activity and recycle stability in 1-hexene epoxidation. The efficient strategy reported in this paper will provide new opportunities for further promoting the industrial application of hollow TS-1.
研究领域:
材料科学
·
催化
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2019
·Vol. 149
·期 4
·974-984
·
IF 2.372
Zhang Xiaotong,He Ning,Liu Chunyan,Guo Hongchen
Highly dispersed Pt–Cu alloy nanoparticles encapsulated in silicalite-1 were prepared by one-pot method. Taking propane dehydrogenation as a probe reaction, it was found that anti-coke ability was improved by encapsulation. Through H 2 -TPR, CO adsorption DRIFT spectra and X-ray Photoelectron Spectroscopy experiment, enhanced anti-coke ability was ascribed to the electronic environment change of encapsulated metal. And it was further confirmed by in situ coking experiment. Owning to limited acidity, metal encapsulated by silicalite-1 molecular sieve exhibited better anti-coke ability and higher propylene selectivity than that by stronger acidic ZSM-5 molecular sieve. Moreover it was found that the combination of Cu and Pt made better catalytic performance and accelerated dehydrogenation more effectively compared with monometallic catalysts. Therefore, Pt–Cu alloy nanoparticles encapsulated in silicalite-1 molecular sieve core–shell material was a potential coke-resistant catalyst for alkane dehydrogenation reaction. Graphical Abstract
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Huan Wang,Guo Du,Shaohua Chen,Zhipeng Su,Pingchuan Sun,Tiehong Chen
As an important heterogeneous catalyst , Titanium Silicalite-1 (TS-1) zeolite has been widely applied in various catalytic processes. Here, hierarchical TS-1 single-crystals were successfully synthesized by a steam-assisted crystallization strategy using hierarchically porous titanium-containing silica (Ti-NKM-5) as a precursor. Due to the presence of large mesopores (10–40 nm)， the microporous structure-directing agents penetrated the interstitial structure of silica particles, inducing the dissolution and crystallization process . During crystallization, the generated nanocrystals grew together to form a hierarchical structure. Titanium was fully incorporated into the zeolite framework, and no extra-framework anatase was formed. Compared with the traditional microporous TS-1 zeolite, the synthesized hierarchical TS-1 single-crystal exhibited superior catalytic performance in oxidative desulfurization (ODS) of dibenzothiophene (DBT) and 4, 6-dimethyl dibenzothiophene (4, 6-DMDBT) owing to the hierarchically porous and anatase-free structure. The recycling test revealed the durability of the obtained hierarchical TS-1 catalyst under moderate reaction conditions.
研究领域:
化学
·
材料科学
·
催化
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Dingmei Han,Meiyu Liu,Chengming Huang,Xinyu Sun,Linjie Guan,Binbin He,Yi Mei,Yun Zu
Co-based catalysts are promising alternatives to replace expensive Pt- and toxic Cr-based catalysts for propane dehydrogenation (PDH), while the catalytic stability and propylene selectivity have been subjected to the diversity of Co speciations. Given the situation, uniformly stable hydroxylated Co 2+ silicate sites (depicted as {OH–Si–(OH)–Co–O–Si-(OH) 3 }) are successfully embedded into the silicalite-1 zeolite framework located in the straight and intersection channels (Co@S-1) with the assistance of Co precursors and geminal silanols via a facile hydrothermal synthesis , as revealed by detail characterizations. Under comparable conditions, a superior catalytic PDH performance with attractive propylene formation rate of 14.6 mmol·g cat −1 ·h −1 , propylene selectivity higher than 93% and very low deactivation rate of 0.0206 h −1 after 7 h is achieved over the Co@S-1(EDA) catalyst. Furthermore, the catalytic performance can be restored to the same as that of the fresh catalyst after 3 successive regenerations. In situ FTIR spectra analysis further reveals the dynamic changes in the characteristic absorption bands associated with the hydroxylated Co 2+ silicate sites and the intermediate product (2-propyl) during the PDH reaction and a reaction mechanism is proposed accordingly. This work provides a new insight for designing high-efficiency nonprecious metal PDH catalysts.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
·
2025
·
IF 4
Lizhi Wu,Ying Zhang,Caixin Zou,Qin Sun,Baozhen Li,Wenchun Zheng,Jiamin Liu,Juncheng He,Yu Tang,Li Tan
Ethane dehydrogenation to aromatics (EDA) is one of the most promising routes to produce aromatics. Herein, the tandem of dehydrogenation component and acidic zeolite are prepared and investigated for EDA. Pt/Fe-S-1 coupled with ZSM-5 of Si/Al of 14 via mixing homogeneously shows excellent EDA performance with 54.0% ethane conversion, 61.5% aromatics selectivity as well as a deactivation rate constant of 0.00010 h −1 . According to catalysts characterizations and controlled experiments, it is confirmed the highly dispersed positive Pt δ + species around Fe species over Pt/Fe-S-1 is the active sites for ethane dehydrogenation to ethylene and subsequent naphthenes dehydrogenation to aromatics, Brønsted acid sites of ZSM-5 and MFI pore are responsible for ethylene oligomerization and cyclization to naphthenes and further naphthenes dehydrogenation to aromatics. The short spatial space between dehydrogenation active sites and acid sites is beneficial for EDA. And the ethylene generation rate is the rate-determining step of EDA.
研究领域:
催化化学
·
材料科学
·
能源化工
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Fuwen Yang,Jie Zhang,Jinwei Chen,Gang Wang,Tong Yu,Junyu Zhao,Qian Li,Zongbo Shi,Runsheng Zhuo,Ruilin Wang
Propane dehydrogenation (PDH) provides a promising way to meet the requirement of propylene supply, but the commonly-used Pt-based catalysts still suffer from unsatisfactory stability and deactivation. Herein, an interfacial regulation strategy is developed to construct the Cu, Pt, and Zn species modified hollow porous silicalite-1 (CuPt/Zn-HPS-1). Owing to the regulation role of Pt, the electron-deficient [ZnOH] + Lewis acid sites accelerated the C-H activation, which was beneficial to achieve the excellent PDH performance. More importantly, the additionally introduced Cu 2+ further modulated the geometric structure and electronic density of Pt, thus effectively improving the anti-sintering ability and alleviating the coke deposition. Benefiting from the interfacial regulation and Lewis active [ZnOH] + sites, the optimal CuPt/Zn-HPS-1 catalyst exhibited an excellent catalytic PDH performance with the initial propane conversion of 30.4 % and propylene selectivity of 99.0 %. The CuPt/Zn-HPS-1 also demonstrated robust recycling stability in reaction-regeneration cycling test with the smaller deactivation rate constant. This work affords a strategy for improving PDH performance in practical industrial application.
研究领域:
化学工程
·
催化科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Greenhouse Gases-Science and Technology
·
2024
·Vol. 14
·期 6
·954-976
·
IF 2.7
Xianglian Wu,Aisha Nulahong,Conghui Miao,Qinghua Liu,Jiangyuan Li,Changmin Tuo
In this work, an alkali melting-pickling assisted solid phase synthesis method of S-1 zeolite molecular sieve with excellent adsorption properties for CO 2 was successfully developed by using solid waste fly ash. SiO 2 with a purity of up to 97.84% was successfully extracted by using alkaline fusion activation, high temperature calcination and pickling. The CO 2 adsorption capacity of the prepared SiO 2 was 0.51 mmol/g at 298 K and 1 bar. Silicalite-1 molecular sieve was prepared by solid phase synthesis method using SiO 2 extracted from fly ash as silicon source. The results showed that the prepared Silicalite-1 had good morphology and relatively high crystallinity. The specific surface area is 623.30 m 2 /g, and the total pore volume is 0.31 cm 3 /g. In addition, the adsorption capacity of CO 2 was 2.05 mmol/g at 298 K and 1 bar. Compared with the prepared SiO 2 , the adsorption capacity of CO 2 by Silicalite-1 molecular sieve increased by four times. Moreover, under the test condition of 298 K, it has a high selectivity coefficient for CO 2 /N 2 mixed gas, and after 10 times of adsorption-desorption cycle tests, the adsorption capacity of Silicalite-1 molecular sieve for CO 2 does not change significantly, and its adsorption rate can still be as high as 89.31%. The results indicate that Silicalite-1 molecular sieve prepared by solid phase synthesis method has good adsorption selectivity and adsorption–desorption cycle regeneration stability, and can be used in the field of CO 2 adsorption, separation and purification. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2026
·Vol. 60
·期 30
·21168-21179
·
IF 12.2
Chen Zhiqiang,Xie Xiaoqiang,Zhou Xincheng,Tu Xiang,Zhuo Fengqing,Ji Jian,Yu Fengbo,Li Guobo,Liu Wenming,Wei Lu,Deng Jiguang,Dai Weili,Peng Honggen
Water-induced deactivation of Pd-based
catalysts for
light alkane
combustion remains a significant challenge. Herein, S-1 zeolite-encapsulated
Pd–Pt bimetallic oxide nanoclusters were prepared for catalytic
propane oxidation. The optimized Pd 0.8 Pt 0.2 @S-1
catalyst exhibits exceptional water resistance with the propane oxidation
reaction temperature (T 90 ) shifting by a mere 9 ° C
in the presence of 5% H 2 O and fully recovering once the
water feed is terminated, superior activity, and thermal stability.
Combined experimental and theoretical insights reveal that the introduction
of Pt induces the formation of Pt–O–Pd bonds, modulating
the electronic structure of Pd to enhance surface hydrophobicity,
optimize oxygen and propane adsorption, and promote propane activation. In situ DRIFTS studies further confirm that propane oxidation
over Pd 0.8 Pt 0.2 @S-1 proceeds via a Mars–van
Krevelen mechanism. This work sheds new light on confined bimetallic
synergistic effects for the rational design of catalysts with superior
performance.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Kai Jia,Yihao Zhao,Mingyuan Shao,Fangqi Yu,Yongqing Wang,Shanbing Mao,Zhendong Liu
The demand for zeolites is expected to grow rapidly due to their expanding applications in catalysis and separation, which drives the need for efficient synthesis routes based on economical raw materials. To overcome the limitations of time-consuming conventional zeolite synthesis, an ultrafast and low-cost route has been developed using industrial-grade sodium silicate as the silica source. This approach enables minute-level synthesis of silicalite-1 zeolite through a combination of acid neutralization and seeding strategies. Notably, carbon dioxide was also demonstrated as an effective neutralizing agent, offering a sustainable alternative. This ultrafast route further enabled the in-situ encapsulation of metal nanoclusters during zeolite crystallization, which resulted in well-defined metal-zeolite catalysts. Using Pt–Zn as a model system, the catalysts exhibited high activity and long-term stability in propane dehydrogenation. This work presents a scalable and economical route for producing high-performance zeolite catalysts and highlights the potential for broader application in commercial dehydrogenation processes and beyond.
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2026
·
IF 4
Ziheng Li,Junxin Guo,Haoze Liu,Dule Huhe,Zhao Wang
Despite their high methanol selectivity in CO2 hydrogenation, In2O3-based catalysts still face limitations in CO2 conversion and long-term stability. This work addresses these challenges by designing a highly dispersed Pd/In2O3 catalyst supported on self-pillared silicalite-1 (SP-S-1) zeolite. The well-defined channels and abundant surface silanol groups of SP-S-1 effectively anchor and disperse In2O3 nanoparticles. This structure also spatially isolates Pd species, which prevents their sintering and inhibits the formation of inactive Pd–In alloys. Comprehensive characterization reveals that the strong metal-support interaction stabilizes oxygen vacancies and prevents over-reduction of In3+ species, which are crucial for CO2 activation and methanol selectivity. The optimized Pd/In2O3/SP-S-1 catalyst achieves a methanol space-time yield of 2.57 gMeOH·gIn+Pd-1·h-1 at 300 °C, approximately five times higher than that of the unsupported counterpart. More importantly, it demonstrates high stability, retaining 95% of its initial activity after 100 hours on stream, far outperforming the unsupported catalyst. This work highlights zeolite confinement as a versatile strategy for designing robust and efficient CO2-to-methanol catalysts.
✓ 已验证
产品关联
DOI
高影响因子
CRYSTAL GROWTH & DESIGN
·
2026
·
IF 3.4
Ruilan Xu,Junhui Cai,Kaipeng Zhang,Yongxuan Wang,Jingjing Kou,Xintu Lin,Lu Gan,Shangxi Zhang,Zhengbao Wang,Yong Peng
Hollow-structured MFI zeolite exhibits great potential as a high-performance catalyst, adsorbent, and low-k material. For the construction of interior voids in silicalite-1 (pure silica MFI-type) zeolite, alkaline etching by TPAOH aqueous solution is a typical top-down approach. However, tough conditions like high temperature (around 170 °C) and high pressure (generated in autoclave), which are unfavorable for the safety operation and large-scale application, are necessary for the creation of a hollow structure in the zeolite. In this work, alkaline etching at mild conditions of typically 80 °C and atmospheric pressure by using TMAOH, TEAOH, and TBAOH as etchants is comparatively investigated in detail on the basis of the preliminary study that concentrated on the TPAOH etchant. Hierarchical hollow silicalite-1 zeolites are successfully obtained at different processing times for TEAOH-/TBAOH-etching, while TMAOH-etching only leads to the formation of plate-like crystals even at relatively harsh treatment conditions. The thinning trend of the wall thickness of hollow silicalite-1 against etching time varies depending on the employed etchant. The adsorption affinity of organocations on the zeolite surface of silicalite-1 decreases in the order TMA+ > TEA+ ≥ TBA+ > TPA+. The protection-dissolution etching mechanism associated with different etchants is analyzed. Two more detailed routes of protection-dissolutioninternal (p-din) and protection-dissolutionexternal (p-dex) are, for the first time, identified for TEAOH/TPAOH/TBAOH and TMAOH, respectively. The zeolite film layers prepared from the hollow silicalite-1 seeds possess internal cavities, exhibiting good anticorrosion ability and low dielectric constant k values.
✓ 已验证
产品关联
DOI
高影响因子
Polymers
·
2022
·Vol. 14
·期 9
·1680
·
IF 4.967
Qiuping He,Wei Chen,Pengfei Wang,Xiaoming Dou
Separation of dichlorobenzene (DCB) isomers with high purity by time− and energy−saving methods from their mixtures is still a great challenge in the fine chemical industry. Herein, silicalite-1 zeolites/polydimethylsiloxane (PDMS) hybrid membranes (silicalite-1/PDMS) have been successfully fabricated on the porous polyvinylidene fluoride (PVDF) supports to first investigate the pervaporation separation properties of DCB isomers. The morphology and structure of the silicalite-1 zeolites and the silicalite-1/PDMS/PVDF hybrid membranes were characterized by XRD, FTIR, SEM and BET. The results showed that the active silicalite-1/PDMS layers were dense and continuous without any longitudinal cracks and other defects with the silicalite-1 zeolites content no more than 10%. When the silicalite-1 zeolites content exceeded 10%, the surfaces of the active silicalite-1/PDMS layers became rougher, and silicalite-1 zeolites aggregated to form pile pores. The pervaporation experiments both in single-isomer and binary−isomer systems for the separation of DCB isomers was further carried out at 60 °C. The results showed that the silicalite-1/PDMS/PVDF hybrid membranes with 10% silicalite-1 zeolites content had better DCB selective separation performance than the silicalite-1/α−Al2O3membranes prepared by template method. The permeate fluxes of the DCB isomers increased in the order of m−DCB < o−DCB < p−DCB both in single-isomer and binary-isomers solutions for the silicalite-1/PDMS/PVDF hybrid membranes. The separation factor of the silicalite-1/PDMS/PVDF hybrid membranes for p/o−DCB was 2.9 and for p/m−DCB was 4.6 in binary system. The permeate fluxes of the silicalite-1/PDMS/PVDF hybrid membranes for p−DCB in p/o−DCB and p/m−DCB binary−isomers solutions were 126.2 g∙m−2∙h−1and 104.3 g∙m−2∙h−1, respectively. The thickness−normalized pervaporation separation index in p/o−DCB binary−isomers solutions was 4.20 μm∙kg∙m−2∙h−1and in p/m−DCB binary−isomers solutions was 6.57 μm∙kg∙m−2∙h−1. The results demonstrated that the silicalite-1/PDMS/PVDF hybrid membranes had great potential for pervaporation separation of DCB from their mixtures.
研究领域:
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）